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Hydrogen production for energy: An overview

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DOI: 10.1016/j.ijhydene.2019.12.059

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Review Article

Hydrogen production for energy: An overview

Furat Dawood*, Martin Anda, G.M. Shafiullah

College of Science, Health, Engineering and Education, Murdoch University, Perth, WA, Australia

highlights graphical abstract

Innovative hydrogen cycle model

proposed of a square-shaped
Hydrogen Square (HydS).

Innovative HPP categorising model
proposed to describe the H2 pro-
duction pathways. .

The cost of the hydrogen purifica-
tion must be added to the
hydrogen cycle feasibility.

The guarantee of hydrogen origin
is essential to ensure its energy
cleanness.

An innovative hydrogen cleanness
index model has been introduced.

article info abstract

Article history: Power to hydrogen is a promising solution for storing variable Renewable Energy (RE) to
Received 15 September 2019 achieve a 100% renewable and sustainable hydrogen economy. The hydrogen-based energy
Received in revised form system (energy to hydrogen to energy) comprises four main stages; production, storage,
26 November 2019 safety and utilisation. The hydrogen-based energy system is presented as four corners
Accepted 10 December 2019 (stages) of a square shaped integrated whole to demonstrate the interconnection and
Available online 11 January 2020 interdependency of these main stages. The hydrogen production pathway and specific
technology selection are dependent on the type of energy and feedstock available as well as
Keywords: the end-use purity required. Hence, purification technologies are included in the produc-
Hydrogen square tion pathways for system integration, energy storage, utilisation or RE export. Hydrogen
Hydrogen production production pathways and associated technologies are reviewed in this paper for their
Hydrogen economy interconnection and interdependence on the other corners of the hydrogen square.
Hydrogen cleanness index Despite hydrogen being zero-carbon-emission energy at the end-use point, it depends
on the cleanness of the production pathway and the energy used to produce it. Thus, the
guarantee of hydrogen origin is essential to consider hydrogen as clean energy. An

Abbreviations: RE, Renewable Energy; HydESS, Hydrogen-based Energy Storage Systems; HydS, Hydrogen Square model; LCA, Life
Cycle Assessment; H2X, Hydrogen to X; CCS, Carbon Capture and Storage; HPP, Hydrogen Production Pathway; Capex and Opex, Capital
cost and Operating cost; HCI, Hydrogen Cleanness Index.
* Corresponding author.,
E-mail address: Furat.Dawood@murdoch.edu.au (F. Dawood).
https://doi.org/10.1016/j.ijhydene.2019.12.059
0360-3199/© 2019 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.
3848 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 5 ( 2 0 2 0 ) 3 8 4 7 e3 8 6 9

innovative model is introduced as a hydrogen cleanness index coding for further investi-
gation and development.
© 2019 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.

Contents

Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3848
Hydrogen . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3849
Hydrogen history and historical accidents . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3849
How safe is hydrogen . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3851
Hydrogen properties . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3851
Hydrogen economy . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3851
Hydrogen production (HydS 1st corner) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3853
Hydrogen production pathways . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3853
Emerging hydrogen production technologies . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3854
Hydrogen purity grading model . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3854
Innovative hydrogen cleanness index model . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3857
Discussion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3859
Conclusion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3860
Acknowledgment . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3860
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3860

Hydrogen-based Energy Storage Systems (HydESS) is gaining

Introduction
The continuous growth of the world population and economy,
coupled with rapid urbanisation has resulted in a monu-
mental increase in energy demand [1e5]. The classic trend of
energy supply depends on hydrocarbon (fossil fuel) energy
resources which, are depleted and limited by geographical
distribution and ease of extraction [6e8]. The ways by which
we have utilised fossil fuels as our principal source of energy
since the industrial revolution have caused a massive increase
in the levels of CO2 and other Greenhouse Gases (GHG) in our
atmosphere which is the main cause of global warming
[8e11]. Thus, decarbonisation of the energy supply by utilising
alternative clean, sustainable and renewable energy is
essential for future energy sustainability and global security
[5,10,12e15].
Renewable Energy (RE) resources will play a key role in the
transition towards a clean and sustainable energy system
[16,17]. The main challenge in transitioning towards 100% RE
is the variable and intermittent nature of these resources
[14,18e20]. This requires technical adaptation, in particular
relating to balancing variable supply and varying demand for
energy [6,21,22]. The increase in renewable energy penetra-
tion into the current energy systems raises the need for large-
scale energy storage systems to deal with the RE sources’
variability and intermittency [6,23e25]. The storage systems
will need to decouple supply and demand by shifting the
generated energy on different time scales (hourly, daily and
seasonally) [20,26e28].
The elegant idea of storing RE in an energy carrier such as
hydrogen [10,11,17,29], which is storable, transportable and
utilisable can be the solution [10,30]. Hence, the concept of a
potential as a cost-effective solution for large-scale RE storage,
transport and export [10,29,31e33]. The literature reveals that
HydESS are leading the way towards a 100% renewable energy
economy which is called the hydrogen economy [10,29,33].
Therefore, there is a growing body of literature that recognises
the importance of HydESS and of utilising hydrogen as an
energy carrier to enable the shift to carbon-free energy gen-
eration and utilisation [10,34,35]. However, the majority of the
literature showed that a full hydrogen dependent economy is
still highly debatable and not yet realisable [34,36e43],
although it has recently started to gain potential [35,44e51].
Hydrogen can be produced from a wide range of resources
using different feedstock, pathways and technologies,
including fossil fuels and RE resources [7,8,10,15,49,52,53]. The
classic method is by cracking or reforming fossil fuel as a cost-
effective hydrogen production pathway for industrial use
which is estimated (globally) at 85 million tonnes in 2016 (over
600 Billion Nm3/yr) [10,54]. Thus, hydrogen energy value and
clean energy index (cleanness) were not the main factors to
account for, rather than hydrogen as a feedstock material i.e.
industrial raw commodity which is called industrial hydrogen
[11,55,56]. The industrial hydrogen was used for fertiliser
production [57e60], petrochemical refining [60e63], metal
work [56,61,64], food processing [50,58,65e68], power gener-
ator cooling in power plants [11] and semiconductor
manufacturing [11]. Meanwhile, with growing attention being
paid to reducing GHG emissions, RE resources start rapidly
gaining potential as a clean source to produce hydrogen
(renewable hydrogen) as a carbon-emissions-free energy
carrier [56,58,69e71]. The renewable hydrogen creates the link
between RE resources and the modernisation of energy sup-
ply, transport, industry and RE energy export [7,10,62,72]. A
 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 5 ( 2 0 2 0 ) 3 8 4 7 e3 8 6 9
hydrogen-based energy system is not less resilient than the
conventional fossil fuel based system as hydrogen can be used
as direct fuel (pure H2 or fuel admixture) or converted to other
liquid/gas fuels [58,61,73e76].
Based on the extensive literature review this study identi-
fied that the hydrogen-based energy system comprises mainly
four main stages (corners), which are interconnected and
interdependent [7,8,10,11,15,56,77e80]. These four stages are
hydrogen production, storage, safety and utilisation with
which this study proposed a four corners model, named
Hydrogen Square (HydS) as shown in Fig. 1. The proposed
innovative HydS model illustrates the interdependence of
each stage on the other stages which must be considered in
any pathway selection. The term HydS will be used onward in
this paper to refer to the complete cycle of hydrogen uti-
lisation in the energy systems and interconnections between
the four corners (stages). The two sub-stage (sub-systems)
processes namely hydrogen purification and compression,
can be in any of the HydS corners as shown in the centre of the
HydS in Fig. 1. The purification and compression sub-systems
costs (energy consumption and recovery rate) must be taken
into account in selecting the production pathway (decision
making) as well as the Life Cycle Assessment (LCA) process,
which are discussed in detail in the following sections of this
paper.
A comprehensive literature review has been conducted in
this paper to identify state-of-the-art research and projects in
the HydS pathways and technologies. The most recent and
relevant publications in the hydrogen energy field are sum-
marised in Table 1.
An exploration of the published Research and Develop-
ment (R&D) literature in Table 1, reveals that there is no one
article, research study or book that covers the four corners
interdependence of the HydS. Likewise, there is no clear
connection between hydrogen purification cost and the
Fig. 1 e The proposed Hydrogen Square (HydS): four
corners model.
3849
production pathways. Instead, most of the reviewed refer-
ences focussed on one corner and sometimes touching briefly
on the other corners. Furthermore, many comprehensive
studies were conducted in the hydrogen production corner
(HydS first corner) with a focus on one pathway
[30,44,58,64,67,68,72,81e91,93e106]. The review of the edited
books [7,8,56,78] offered a more detailed overview of one or
more corners of the HydS or covering the four corners but,
within the boundaries of a specific perspective
[20,32,141e153]. A large number of papers in the literature
were giving inclusive background information in one or more
of the HydS corners, however, with focus on modifying or
improving a specific area or technology as shown in Table 1,
[14,20,22,27,32,45,46,82
[14,20,22,27,32,45,46,82,110e140,141e153,155e178]. Hence, it
is noticeable that most of the literature are not yet connecting
the storage technologies and the end-use of hydrogen to the
production pathways as well as the case-specific safety
guidelines.
This review paper provides an overview of hydrogen’s role
in the energy sector and the transition towards 100% renew-
able, sustainable, green energy. The present paper seeks to
integrate the research findings in hydrogen production path-
ways and associated technologies in connection with the
wider picture of the HydS. The discussion section in this paper
is limited to hydrogen production for the energy sector only.
One of the main contributions of this review paper, therefore,
is to provide insights regarding into the planning of hydrogen
production systems through awareness of the four corners of
HydS pathways. Various hydrogen production pathways and
technologies are discussed from the perspective of each of the
other HydS corners rather than focusing on cost-effectiveness
of the production pathways only.
Hydrogen
Hydrogen (H2) is the most abundant element in the universe,
which is found on our planet earth mainly in water and
organic compounds [16,18]. It is the lightest and simplest
element which consists of one electron and one proton [16],
colourless, odourless, flammable gas [197]. Hydrogen’s atomic
weight is 1.00794 atomic mass units rounded at 1.008. This
atomic weight number (1.008) was considered in the USA as
the 8th of October (10/08) as the National Hydrogen and Fuel
Cell Day [207]. This event was first recognised by the Fuel Cell
and Hydrogen Energy Association in 2015 to raise awareness
of fuel cell and hydrogen technologies as well as the vast po-
tential the technologies have today and in the future as shown
in Fig. 2. This day is expected to be the International day of
hydrogen energy.
Hydrogen history and historical accidents
Hydrogen is a material that has been known for more than 200
years. At the beginning of the sixteenth century, Paracelsus
from Switzerland discovered that gas was formed during the
reaction between sulfuric acid and iron [56]. Myelin, also from
Switzerland, reported in the seventeenth century that this gas
burned [56]. In 1761, Robert Boyle produced hydrogen from
3850 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 5 ( 2 0 2 0 ) 3 8 4 7 e3 8 6 9

Table 1 e The recent literature on R&D in the HydS for energy; cited in this paper.
References Corners Covered Scope (focus)
1 2 3 4 *P
Reviews [81,82] 7 7 Ammonia as a hydrogen storage and transport medium
[83,84] 7 7 7 Energy management strategies with hydrogen backup
[85e87] 7 7 7 One type of water electrolysis in focus
[88e92] 7 7 7 7 Hydrogen production via chemical/Bio technologies
[72,93] 7 7 7 Power-to-Methane
[67,94,95] 7 7 7 Water electrolysis technologies for power to hydrogen
[30,44,96e98] 7 7 7 Energy storage with a focus on Power to Gas
[58,68,99e106] 7 7 Hydrogen production and storage technologies
[64] 7 H2 handling and safety (codes and regulations)
[107,108] 7 Purification techniques
Books [8,78] 7 7 7 Fuel Cell technologies, FC fuels and safety (eBook)
[56] 7 7 7 7 H2 energy engineering; A Japanese Perspective (eBook)
[7] 7 Hydrogen storage technologies (eBook)
[109] 7 Purification techniques
Articles [110,111] 7 Specific type of electrolyser
[112e125] 7 Specific type of storage
[126e134] 7 Hydrogen Safety (general/specific)
[82,135e140] 7 Hydrogen Utilisation (pathways/specific)
[20,32,141e154] 7 7 7 Case study
[45,155e160] 7 Production by electrolysis (technologies/improvement)
[46,161e163] 7 Chemical hydrogen Production (technologies/improvement)
[14,164e174] 7 Biological/Photosynthesis hydrogen production
[22,27,175e178] 7 Hydrogen-based energy storage systems modelling
[179e186] 7 Purification techniques
Reports [13,60,76,187e189] 7 7 7 National Hydrogen Roadmaps e specific country/region
[190,191] 7 Utilisation/Pathways
[192,193] 7 7 Power-to-Gas
[194e198] 7 Safety, Codes and Regulations
[59,199] 7 7 7 Techno-economic assessment
[200] 7 Purification standards
Innovations [95,201,202] 7 7 Unitized reversible/regenerative hydrogen
[203,204] 7 7 Battolyser
[205] 7 7 Residential fuel cells for hydrogen supply for FCEVs
[74,206] 7 Membraneless Electrolysers
[7,54,105] 7 Electrochemical compression

*P ¼ Covering hydrogen purity techniques.

reacting iron filings and dilute acids [197]. In 1776, Henry
Cavendish identified hydrogen as a unique substance and he
was named as the discoverer of hydrogen because he reported
key findings in an article to the Royal Society of London
[10,56,78,197]. In 1783, Antoine Lavoisier produced hydrogen
[197], and in 1788 he named the material hydrogen (Hydro-
genium) from the Greek roots “hydro” (water) [10]. In 1800, the
English Nicholson and Carlisle used for the first time the
electrolysis of water to produce it [10,56]. It was liquefied by
James Dewar in 1898 [10]. In 1839 a British scientist, Sir Wil-
liam Robert Grove, developed the first hydrogen-powered fuel
cell [197]. Count Ferdinand von Zeppelin of Germany invented
the first balloon in 1900 that used hydrogen to maintain the
buoyancy of an airframe [56]. Airships to cross the Atlantic
were put into service during the 1920s and 1930s [56]. In the
U.S., NASA was founded in 1958 to pursue space exploration
and made great historical contributions to hydrogen use. It
employed hydrogen as a fuel and was the world’s largest
liquid hydrogen user by 1961 [56]. The first space shuttle was
launched in 1981, and the Soviet Union completed a flight with
TU-155, the world’s first jet engine aircraft that used liquid
hydrogen fuel, in 1988 [56].
Hydrogen has often been synonymous with danger due to
its extremely flammable nature [137,197] especially since the

Fig. 2 e Hydrogen chemical element and USA National Hydrogen and Fuel Cell Day, picture modified from: http://www.
fchea.org/h2-day-2018.
 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 5 ( 2 0 2 0 ) 3 8 4 7 e3 8 6 9
Fig. 3 e Hydrogen historic accidents; Source: https://www.airships.net/hydrogen-airship-accidents/, a. Hindenburg, while
on fire, b. Wreck of LZ-10 Schwaben at Düsseldorf, c. Airship Roma after ignition.
Hindenburg disaster on May 6, 1937 which killed 35 of the 97
passengers on the airship [208] and the following accidents as
shown in Fig. 3.
Although, analysis of the origin of some hydrogen acci-
dents show that “organizational and human factors”
contributed to the causes most of these accidents (in over 70%)
[194], these accidents have been the causes of people strug-
gling to effectively manage hydrogen [194,208].
How safe is hydrogen
Hydrogen is non-toxic and much lighter than air, it dissipates
rapidly when it is released, allowing for relatively rapid
dispersal of the fuel in case of a leak which makes it relatively
safer than other spilt fuels [209]. The primary safety concern is
that if a leak goes undetected and the gas collects in a confined
space, it can eventually ignite and cause an explosion [210].
Hydrogen as a fuel, like all fuels, has some degree of danger
thus, the safe use of any fuel focuses on preventing situations
where the three combustion factors; ignition, oxidant and fuel
are present [209]. However, some of hydrogen’s properties
require additional engineering controls to ensure its safe use;
like a wide range of flammable concentrations in air (4%e75%)
and lower ignition energy (only one 10th as much energy to
ignite as gasoline) [8,211]. In addition, metal hydrogen
embrittlement and ability to damage materials in point of leak
require attention in materials selection for the HydS system
[8,56,64,76,132,137,193,196e198,209,212]. A thorough under-
standing of hydrogen properties and designing safety features
into hydrogen systems, training in safe hydrogen storing and
handling practices are key elements for ensuring the safe use
of hydrogen [8,56,64,76,137,193,196e198].
The USA Department of Energy stated in its website [209]
“As more and more hydrogen demonstrations get underway,
hydrogen’s safety record can grow and build confidence that
hydrogen can be as safe as the fuels in widespread use today”.
Hydrogen properties
Hydrogen energy content at the higher heating value is
141.8 MJ/kg at 298 K and the lower heating value of the
hydrogen is 120 MJ/kg at 298 K, which is much higher than that
3851
of most fuels (e.g., gasoline 44 MJ/kg at 298 K) [85,137,213,214].
However, liquid hydrogen has less energy density by volume
than hydrocarbon fuels such as gasoline by approximately a
factor of four (i.e. density of 8 MJ/l whereas gasoline has a
density of 32 MJ/l) [123,215]. While, hydrogen gas has good
energy density by weight, but poor energy density by volume
versus hydrocarbons, therefore it requires a larger tank to
store [123,127]. Hydrogen is a flammable gas with relatively
low ignition temperature which creates a large portion of the
risk associated with its usage [197]. Also, it has the ability to
escape through materials due to its small molecule size and its
destructive capability (hydrogen embrittlement) which can
lead to mechanical degradation and failure to the point of
leakage in certain materials [8,56,64,76,132,193,196e198,212].
A hovering overview of hydrogen properties and specifica-
tions is given in Table 2 below to demonstrate the opportu-
nities and technical challenges in the proposed HydS.
Hydrogen economy
It seems like every day there is a new announcement about
hydrogen for energy utilisation and automobility. The promises
are tantalizing, since Hydrogen to X (H2X) has the potential to
very quickly integrate into the existing energy and transport
systems while significantly reducing air pollution (zero-carbon-
emission at point of use) [10,11,17,29,47]. At the same time,
everything from oil spills to ozone alerts to global warming gets
blamed on our dependence on fossil fuels [5,10,12e15,48]. The
security of energy supply and price stability are also high on the
political agenda [6e8]. These forces are leading the world’s shift
away from the fossil fuel economy toward a much cleaner
hydrogen future what is broadly known as the hydrogen
economy since firstly proposed at the beginning of 1970’s “at
General Motors (GM) Technical Centre by “John Bockris” and
Miami meeting on hydrogen” [33,63,218,219]. The literature
shows that the hydrogen economy has been actively investi-
gated; many reviews and case studies have been prepared as
well as many roadmap reports were published highlighting key
progress made and the role of the prospect of hydrogen within
the energy sector [8,17,29,32,35,58,63,76,77,220]. Peer-reviewed
research in the literature shows growing interest in discus-
sing the techno-economic, environmental impact, policy
3852 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 5 ( 2 0 2 0 ) 3 8 4 7 e3 8 6 9

Table 2 e Hydrogen properties and specifications.

Properties SI Units References
Discovery date/by/Chemical formula 1766/Henry Cavendish/H2 [216]
1
Isotopes H (99.98%), 2H, 3H, [216]
(4He7H Unstable)
Equivalences; Hydrogen solid, liquid and Gas 1 kg ¼ 14,104 l ¼ 12,126 m3 [194]
at Pressure ¼ 981 mbar and Temperature ¼ 20  C
Molecular weight 1.00794 [8,197]
Vapor pressure at (252.8  C) 101.283 kPa [8,197]
Density of the gas at boiling point and 1 atm 1.331 kg/m3 [8,197]
Specific gravity of the gas at 0  C and 1 atm (air ¼ 1) 0.0696 [8,197,217]
Specific volume of the gas at 21.1  C and 1 atm 11.99 m3/kg [8,197]
Specific gravity of the liquid at boiling point and 1 atm 0.0710 [197]
Density of the liquid at boiling point and 1 atm 67.76 kg/m3 [197]
Boiling point at (101.283 kPa) 252.8  C [197]
Freezing/Melting point at (101.283 kPa) 259.2  C [8,197]
Critical temperature 239.9  C [197]
Critical pressure 1296.212 kPa, abs [197]
Critical density 30.12 kg/m3 [197]
Triple point 259.3  C at 7.042 kPa, abs [8,197]
Latent heat of fusion at the triple point 58.09 kJ/kg [197]
Latent heat of vaporization at boiling point 445.6 kJ/kg [197]
Solubility in water vol/vol at 15.6  C 0.019 [197]
Dilute gas viscosity at 26  C (299 K) 9  106 Pa s [211]
Molecular diffusivity in air 6.1  105 m2/s [211]
Cp 14.34 kJ/(kg) ( C) [137,197]
Cv 10.12 kJ/(kg) ( C) [197]
Ratio of specific heats (Cp/Cv) 1.42 [197,211]
Lower heating value, weight basis 120 MJ/kg [211]
Higher heating value, weight basis 141.8 MJ/kg [211]
Lower heating value, volume basis at 1 atm 11 MJ/m3 [211]
Higher heating value, volume basis at 1 atm 13 MJ/m3 [211]
Stoichiometric air-to-fuel ratio at 27  C and 1 atm 34.2 kg/kg [137]
Flammable limits in air 4%e75% [137,197]
Explosive (detonability) limits 18.2 to 58.9 vol% in air [211]
Maximum combustion rate in air 2.7/3.46 (m s1) [8]/[194]
Maximum flame temperature 1526.85  C [211]
Autoignition temperature/in air 400  C/571  C [197]/[8,211]

aspects and social implications of hydrogen economy for the advance readiness for hydrogen economy era. Some examples
sake of completeness [2,17,29,65]. Therefore, many national are tabulated in Table 3 below.
and international bodies have been formed to educate the In the literature at a global scale, the hydrogen economy is
public, industries and policy makers to build a framework and not proposed as an alternative to traditional energy vectors

Table 3 e National and International hydrogen frameworks, organizations and councilsa.

Body Location website
IEA Hydrogen Global http://ieahydrogen.org/
Hydrogen Council Global http://hydrogencouncil.com/
The International Centre for Hydrogen Energy UNIDO https://www.unido.org/
Technologies (ICHET)
International Association for Hydrogen Energy (IAHE) Global http://www.iahe.org/
Hydrogen Foundation Spain http://hidrogenoaragon.org/en/
Hydrogen Europe Europe https://hydrogeneurope.eu/
National Hydrogen Association (NHA) USA http://www.hydrogenassociation.org/
The Fuel Cell and Hydrogen Energy Association (FCHEA) USA/Global http://www.fchea.org/
The Hydrogen South Africa (HySA) Africa https://www.hysa-padep.co.za/
Renewable Hydrogen Council WA-Australia http://www.drd.wa.gov.au/projects/
EnergyFutures/Pages/Renewable-Hydrogen-Conference.aspx
The Australian Association for Hydrogen Energy (AAHE) Australia http://www.hydrogenaustralia.org/
The U.S. DOE Hydrogen and Fuel Cells Program USA https://www.nrel.gov/hydrogen/
Canadian hydrogen and fuel cell industry Canada http://www.chfca.ca/
a
This table includes some examples; while there are many other national level entities and think tanks working in the same direction.
 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 5 ( 2 0 2 0 ) 3 8 4 7 e3 8 6 9
but rather as a compliment in the context of a smart and low
carbon strategy for specific applications and locations
[17,35,221]. Therefore, the transition towards global ‘hydrogen
economy’ is not expected to take place within a few years
[35,44e51]. However, recent publicly supported R&D efforts,
cost-effectiveness, policies and deployment of a hydrogen
infrastructure will certainly contribute to make this vision a
reality [2,7,35,65,101,219,222e226].
Renewable hydrogen (i.e. Green Hydrogen)
[55,94,187,227,228], production from renewable energy re-
sources as well as the development of all corners of HydS
seems a promising way to comply with a 100% renewable
electric grid and expanding to a 100% renewable energy sup-
ply hence, hydrogen economy [148,218,219,229,230]. The
literature shows consensus on green hydrogen has the po-
tential to decarbonise a large range of industrial applications
or serve as a clean energy carrier for storing renewable energy
and utilised in a variety of applications [47,148,219,229,230].
However, parallel development in the four corners of the HydS
is essential for the green pathways to become techno-
economically feasible.
Hydrogen production (HydS 1st corner)
In this section, a summary of hydrogen production pathways
and technologies has been discussed and compared to
demonstrate the state-of-the-art hydrogen production tech-
niques. Hydrogen production pathways in the literature have
been categorised into four main categories which are elec-
trolysis, photolysis, biolysis and thermolysis
[15,49,50,58,65e67], and further sub-categorised according to
any combined energy types utilised in the process
[11,15,49,50,65,101,231]. Most of the researchers in the
hydrogen production field have considered some of the energy
additives to the process as a catalytic energy to increase the
process efficiency [2,49,63,232]. Moreover, the literature has
considered some secondary energy types like radiation,
plasma and biological energy amongst the main energy cate-
gories for hydrogen production [49,164,233,234]. An extensive
analysis of the literature revealed a strident mix of hydrogen
production pathways according to the energy utilised in the
process and the technology used. Furthermore, the literature
presents ideas for new classifying models for hydrogen sys-
tems (techno-economic assessment) but, not for categorising
the production pathways e.g. 3S and 18S Models [65]. Also,
there is a necessity to recognise the input energy from the
catalyst materials which increases the efficiency of the pro-
cess. Hence, the authors of this literature review have intro-
duced an innovative model to define the category of hydrogen
production pathways which is discussed in the following
section.
Taking another perspective, the literature reveals that
hydrogen cleanness was described and labelled by three main
colours code; grey, blue and green [48,222,235,236]. The colour
of hydrogen is determined only by the type of energy or
additional technology utilised to produce that hydrogen
regardless of deep cleanness assessment
[48,62,78,222,235,236]. Therefore, grey hydrogen is considered
to be polluting type of hydrogen [48,235]. Whilst, blue
3853
hydrogen defines the Carbon Capture and Storage (CCS) in-
clusive in the grey hydrogen [48,57,222,235,237]. The green
hydrogen refers to a 100% renewable energy source for
hydrogen production [48,60,235]. Hence, green hydrogen is
considered to be a clean (low-carbon-emissions) hydrogen
energy [10,48,60,62,78,154]. This raises the question if all
renewable energy resources have lower emissions than blue
method for hydrogen production?
The current colour coding model fails to determine pre-
cisely how clean (low-carbon-emission) is that hydrogen
because it fails to determine how much GHG emitted during
the production process, sub-systems or from the lifecycle of
equipment used. Furthermore, this colour coding is identi-
fying RE or CCS utilisation (energy type/origin) rather than
how clean is the produced hydrogen. Authors of this paper
have identified this uncertainty and inaccurate colour coding
in describing precisely the cleanness of any produced
hydrogen. Moreover, the current superficial colour coding
model fails to describe how deep is that cleanness assess-
ment. Therefore, an innovative colour spectrum concept in a
colour coding model has been introduced to resolve this
imprecise issue in the current colour coding model. The pro-
posed innovative model for assessing hydrogen cleanness has
been discussed in section (5).
Hydrogen production pathways
The diverse methods of hydrogen production drew a lot of
attention in recent years to play a key role in integrating future
energy systems and bridging the transition from fossil-based
energy to a renewable energy economy as shown in Table 1.
The methods of producing hydrogen can determine the
cleanness, cost-effective, efficacy and therefore, feasibility of
any Hydrogen Production Pathway (HPP). The HPP depends on
three elements to be in presence which are; the material that
contains hydrogen (hydrocarbons or non-hydrocarbons), en-
ergy source and catalyst material [11,15,49,50,65,101,231].
Hence, the selection of the HPP is dependent on material type
as feedstock to extract the hydrogen, the scale of production
and available energy resources [10,11,78].
The literature review (Table 1) reveals that the hydrogen
can be produced (1st Corner of HydS) from one or more types
of energy using a relevant technology with suitable catalyst as
illustrated in Fig. 4. The energy required to extract hydrogen
from the materials that contain hydrogen can be electric,
photonic, bioenergy, chemical and heat or any combination of
these energy sources [29,49,50,65,81,155,233,238,239]. The
proposed innovative model in Fig. 4 illustrates the energy
sources and their combination possibilities to apply on
hydrogen-containing material in the presence or absence of a
process catalyst to produce hydrogen that determines HPP
choice [10,15,65,79,80]. The catalyst plays an essential role to
facilitate the process and increases production efficiency
[11,49,50,80]. Therefore, developing an efficient and cost-
effective catalytic material is the most rapidly developing
field of research in the literature
[2,29,49,50,52,65,81,155,233,238e240].
The energy utilised to produce (or extract) hydrogen from
hydrocarbons or non-hydrocarbons stored is the direct energy
or catalytic energy [10,11,15,17]. The efficiency of any HPP is
3854 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 5 ( 2 0 2 0 ) 3 8 4 7 e3 8 6 9
Fig. 4 e The proposed hydrogen production pathways.
determined by the produced hydrogen energy value divided
by the energy used to produce it [11,78]. Whilst, the cost-
effectiveness is determined by the feedstock, catalyst mate-
rials and energy costs plus the net present cost of the tech-
nology equipment Capex and Opex [7,11,68]. The literature
shows a wide range of hydrogen production pathways utilis-
ing types of energy directly or converted to apply on
hydrogen-containing materials in the presence of catalyst
materials as summarised in Table 4. This Table was developed
to compare the state-of-the-art technologies of HPPs from a
new perspective focussed on energy and materials rather than
technology. The hypothesis is that the choice of HPP and
associated technology depends on the energy resources and
the hydrogen-containing materials (feedstock) as well as the
endpoint application [48,49]. For example, to extract hydrogen
from organic waste or a hydrocarbon fuel, then electrolysis is
not the right choice while if the endpoint application is a fuel
cell then bio-hydrogen is not suitable before purification
(extra cost) [7e9,81,88,241].
The literature reveals that membrane reactor technology
is progressively recognised as a promising approach to
diversify clean HPPs from hydrocarbons and hydrogen puri-
fication [81,101,242e248]. The R&D efforts in the field of
membrane reactors are gaining potential as an efficient
alternative technology of the traditional energy-intensive
technologies for producing the ultra-pure H2 required for
fuel cells [184,242,248]. The rapid advancement in the
permeable membranes for separation and purification of
hydrogen from gaseous mixtures has added another dimen-
sion for membrane reactors applications [246]. This technol-
ogy with carbon capture technology constitutes new HPP for
clean H2 production from conventional fuels [246,249].
Furthermore, the process intensification by uniting a
membrane-based separation and a catalytic chemical reac-
tion can reduce the cost and increase the purity of the blue
hydrogen production [249].
The literature in many ways consider ammonia (NH3) as a
source material for hydrogen production by decomposition
(Haber-Bosch process) therefore, it has been included in the
hydrogen production technologies [7,11,15,49,225]. However,
industrial ammonia is produced in the first place from
hydrogen, which makes it a storage medium for hydrogen
rather than a HPP [7,11,15,50,59,68,88,250]. Therefore,
ammonia decomposition was not included in Table 4.
The developing awareness and concerns about the GHG
emissions and global warming drew attention towards the
cleanness, energy content of hydrogen and HPP technologies
[7,50,77,99,251]. Furthermore, the trend is to avoid fossil fuels
and other hydrocarbons as feedstock regardless of the clean-
ness of the produced hydrogen [16,20,35,154,240,252]. Hence,
water electrolysis supplied by RE (which is currently 4e5% of
global hydrogen production) [167] is gaining momentum as a
zero-emission energy [17,20,49,50,63,65,252].
Also, the reducing cost trend [276], the high purity and
absence of unwanted impurity like carbon oxides, sulphate
oxides, etc., favour water electrolysis technologies over all
other technologies [81,85,101,253,288,289]. However, there are
some emerging technologies which have the potential to
accelerate the transition towards the hydrogen economy by
reducing the capital cost and increase production efficiency.
Some of these technologies are summarised in the following
section.
Emerging hydrogen production technologies
The literature review (Tables 1 and 4) reveals some novel ap-
proaches to produce hydrogen in more cost-effective path-
ways via some promising rapidly developing technologies.
The possibility of unitising two of the HydS corners, i.e. pro-
duction and utilisation, to work reversibly (regenerative) add
momentum to HydS and can be a game changer in the near
future [8,232,290e294]. Moreover, the potential to reduce the
noble material catalysts or the structural design can reduce
the hydrogen cost which results in making hydrogen energy
economically competitive as shown in Table 5. This Table (5)
summarises the state-of-the-art development of some
promising novel technologies which have the potential and
need further R&D to reduce cost and increase hydrogen pro-
duction efficiency.
Hydrogen purity grading model
The literature generally defines hydrogen purity as a low
content of other impurities, or their absence if they are un-
wanted constituents [7,8,88,302,303]. However, it is rare in the
literature to find direct connection or inclusion of the
hydrogen purification process and its cost in the hydrogen
Table 4 e Summary of hydrogen production process category, feedstock and technology possibility.
Process Category Energy I/P Feedstock Technology Eff. (%) *Clean (C/N/CCS) **TML (110) References
Hydrocarbons (H)
Non-Hydrocarbons (N)
Electrolysis Electric Water (N) AE 62e82 C 9e10 [11,17,49,50,74,253,254]
Brine (N) PEM 67e84 C 7e9 [106,190,212,255]
SOC 75e90 C 3e5
chlor-alkali NA C 2e42e4
Electro-photolysis Electric-Photonic Water (N) Photoelectrochemical 0.5e12 C 1e2 [8,9,11,43,49,50,233,256,257]
Photolysis Photonic Water (N)/Algae (H) Photosynthesis 1.6e5 C/N 1e3 [2,10,11,49,171]

i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 5 ( 2 0 2 0 ) 3 8 4 7 e3 8 6 9
Biophotolysis Bioenergy Microalgae Photo-fermentation <1 N 1e3 [9,11,43,49,68,99,258e260]
Photonic Cyanobacteria Algal Hydrogen 1e3 N 1e3 [260]
Photosynthetic-Bacteria 2e7 N 1e3 [2,50,259e261]
Fat (H) 12e14 N 1e3
Nutrients (H) C/N 1e3
Waste (H)/Biomass (H)
Bioelectrolysis Bioenergy Biomass (H) Microbial electrolysis 70e80 N 1e3 [49,101]
Electric Hydrogenases Nitrogen fixation 10 [262]
Biolysis Bioenergy Microorganism Dark fermentation 60e80 N 3e5 [35,101]
Fermentative bacterias Hydrolysis NA N 2e4 [155,239,258]
Biomass (H)þWater (N) Aqueous phase reforming 35e55 N 5e7 [49,263]
CO (N) þ Water (N) Biological Shift Reaction NA N 2e4 [264]
Bio-thermolysis Bioenergy-Heat Biomass (H) (microwave) acid pretreated Co-fermentation hydrothermal NA N 2e4 [265,266]
35e45 N 1e3 [266e269]
Thermolysis Heat Water (N) Waterthermolysis 20e55 C 1e3 [11,49,99,101,165,270]
Biomass (H) (absence of O2) Pyrolysis 35e50 N 8e10 [88,101]
Biomass (H) Gasification 35e50 N 10 [49,50,68]
Coal (H) Coal gasification 74e85 N/CCS 10 [35]
Fuels (H) Steam Reforming (SR) 60e85 N/CCS 10 [242,244,245,271e274]
Fuels (H) Membrane Reactors 64e90 N/CCS 7e9 [10,88,101,238]
Biomass (H) Partial oxidation 60e75 N 7e9 [11,49,68,101]
Methane (H)þCO2 Autothermal 60e75 N 6e8 [8,49,68,88,101]
CO2 Dry Reforming NA C/N [11,238,275]
Thermo-electrolysis Heat-Electric Fuels (H) Plasma Reforming 9e85 N 1e3 [7,10,49,232,276,277]
Chemical Chemical reaction Water (N) Redox 3-5 wt C 4e6 [2,125,278e280]
Metals (N) NA C 4e6 [2,278,281]
Metal Hydrides (N) NA C/N
Gas-based hydrides (N) NA C
Metal Hydroxides (N)
Radiolysis Radiation Hydrogen peroxide (H2O2) Radiolysis NA C 1e3 [50,282e285]
g-radiolysis

*Cleanness ¼ Clean with no emissions (C). Non-clean with emissions (N). Quasi-clean by using Carbon Capture and Storage (CCS).
**Technology maturity level (TML) has been used in the literature as a modified and consolidated rating scale (110) of both the globally accepted benchmarking tool of Technology Readiness Level
(TRL) and the ARENA developed Commercial Readiness Index (CRI) (a), to help communicate the level of maturity of the particular technology. Levels (110) are adopted similarly to “Beca Pty Ltd”
report prepared for the Australian Renewable Energy Agency (ARENA) in November 2015 [286]. Level 1 refers to basic technology research and level 10 refers to the bankable asset class.
(a) Technology readiness level (TRL) (b) methodology was developed by NASA in the 1970s and since then it has been used in a wide range of sectors, including the energy sector. The index is used for

3855
tracking the progress of technologies (1e9), from applied research (TRL1) to successful system operation in its operating environment (TRL9) [187].
(b) ARENA has developed the Commercial Readiness Index (CRI) as a tool that project proponents may want to use when considering their projects and ARENA will use to measure the “commercial
readiness” (1e6) of renewable energy solutions [287].
3856 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 5 ( 2 0 2 0 ) 3 8 4 7 e3 8 6 9

Table 5 e Emerging hydrogen production technologies.

Technology
Anion Exchange Membrane
(AEM)
Membraneless electrolyser
Membrane Reactor
Photosynthesis
Photocatalytic generation
Dark fermentation followed
by photo-fermentation
Plasma arc decomposition
Unitized Regenerative
Battolyser
Brief Description Current Eff. (%) R&D Area References
Semipermeable membrane designed to 67e74 Catalyst [56,85,86,295,296]
conduct anions while being impermeable Membrane
to gases such as oxygen or hydrogen Efficiency
Two independent laminar flow streams 40e80 Increase pressure [11,74,106,254,255,297]
can be separated up to a certain length, Scale
which ensures the formation of a virtual Unitized regenerative
layer separating anode and cathode Efficiency
A membrane is a mass selectivity 64e90 Membrane [184,246,248,272,298]
structure. Membrane reactor allows CCS
hydrogen transfer under a variety of Catalyst
driving forces like pressure, temperature, Process Intensification
electric potential, etc.
Artificial photosynthesis towards solar 1.6e5/10 CO2 Utilisation to Fuel [2,8,50,262,299]/[43]
fuels generation via CO2 reduction Carbohydrate (food)
Semiconductor-based photocatalytic 3e11 Efficiency [8,43,300]
hydrogen generation by high-energy Catalyst
photons to drive the reaction Integration with PV
Fermentation process followed by second 57 Waste to bio-hydrogen [100,193]
stage activated by exposure to light Catalyst
Efficiency
Natural gas is passed through plasma arc 9e85 Graphite production [49,231,270]
to generate H2 and carbon soot (high- Catalyst
temperature pyrolysis)
Reversible electrolyser and FC in one unit 43e51 Efficiency [8,202,232,290]
i.e. can generate hydrogen and power Round trip Scale
(small scale is available) Switching time
Batteries which can produce hydrogen 76-90 overall Efficiency [203,204,301]
after fully charged H2 production control

production’s techno-economic assessment (referring to Table
1). Therefore, the additional cost of purification must be taken
into account to comply with the end point application speci-
fications. In this section the importance of hydrogen purity in
connection with endpoint applications is discussed to fill this
gap in the literature.
In the literature, the term “number of nines” is used to
indicate the purity e.g. three nines means 99.9% purity or 3.0
in abbreviated decimal fraction, while six nines indicate the
purity of 99.9999% or 6.0 [302,303]. Therefore, the expression
4.6 indicates a four nines purity followed by a 6 i.e. 99.996%
pure [302,303]. This means that the process of expressing the
purity is obtained indirectly through subtraction from one
hundred percent, represent all impurities or contaminants
remaining within the hydrogen gas [302]. Defining hydrogen
purity requirements is dependent on the endpoint applica-
tion as in some specific applications there are technical
constraints on the presence of a specific type of impurity not
just its quantity [304]. For example, in order to use bio-
hydrogen, which always contains CO2 [303] that is not
acceptable in a Fuel Cell and must be removed
(<2 mmol mol1) [179,303].
Hence, a specifications like that of the International Orga-
nization for Standardisation ISO 14,687e2 provides a list of 13
different impurities [305e308] with associated maximum
limits that must not be exceeded when providing hydrogen to
a fuel cell vehicle [303,304,309,310]. Thus, ISO 14,687 was
developed for hydrogen purity specifications depending on
the endpoint applications [304,311,312]. This norm for the
quality of combustible hydrogen IRAM-ISO 14,687:2003 was
originally published in 1999 and corrected in 2001 [313]. The
norm classifies combustible hydrogen in three types, I, II, and
III for gaseous, liquid and ‘‘slush’’ hydrogen, respectively
[308,311,313,314]. The ISO 14,687 has subdivided each type to
purity grades, and further to categories in some grades ac-
cording to the hydrogen end use (utilisation) [311,313]. A
general overview of the ISO 14,687 model summarised in
Table 6.
Furthermore, the ISO developed fuel quality specifications
for hydrogen in response to the widespread deployment of
hydrogen-fuelled fuel cell vehicles. For this purpose, the
technical specification was developed and published; in three
parts as follows [311,315];

Part 1 (ISO 14,687e1): All applications except proton ex-
change membrane (PEM) fuel cells for road vehicles. This
standard is no longer used [311].

Part 2 (ISO 14,687e2) in 2012: Hydrogen Fuel - Product
Specification: Proton exchange membrane (PEM) fuel cell
applications for road vehicles.

Part 3 (ISO 14,687e3) in 2014: Hydrogen Fuel - Product
Specification: Proton exchange membrane (PEM) fuel cell
applications for stationary appliances.
A list of the allowable limits for critical contaminants in
hydrogen fuel (>99.97 purity) for Fuel Cells tabulated in Table
7; according to standards SAE J2719 (Society of Automotive
Engineers) and ISO 14,687e2 [305e308].
Additionally, there is a wide range of rapidly growing
hydrogen applications which raised the need for commer-
cially graded hydrogen with specific purity and impurity
content as listed in Table 8.
 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 5 ( 2 0 2 0 ) 3 8 4 7 e3 8 6 9 3857

Table 6 e Fuel hydrogen types, grades and categories of ISO 14,687e2:2012 [302].
H2 type Grade Category Purity Utilisation (Applications)
*(%)
Gaseous (I) A NA 98.00 Internal combustion engines for transport
Residential or commercial applications (All applications except Fuel Cells)
B NA 99.90 Industrial fuel (power generation or heat energy source)
C NA 99.995 Aircraft and space-vehicle ground support systems
D NA 99.97 Fuel Cells for vehicles
E 1 50.0 Fuel Cells for stationary applications (higher Formaldehyde and Formic
acid [314])
2 50.0 (lower Formaldehyde and Formic acid [314])
3 99.9 (lower Formaldehyde and Formic acid [314])
Liquid (II) A NA 99.995 Aircraft and space-vehicle on board propulsion systems and electrical
energy requirements
Land vehicles except Fuel Cells.
D NA 99.97 Fuel Cells for transportation
Slush (III) NA NA 99.995 Aircraft and space-vehicle on board propulsion

*Purity is expressed as a minimum mole fraction.

Recently, the ISO has established a special International HPP depending on the endpoint application purity re-
technical committee ISO/TC 197; which has 14 technical quirements. However, the literature review reveals a gap in
working groups [61]. These groups are developing 15 interna- the knowledge about the cost of the purification process in
tional standards [61] for hydrogen technologies, systems and relation to HPP which, needs to be addressed for an accurate
devices for the production, storage, transport, hydrogen cost-effective assessment for different pathways. Further-
refuelling stations, measurement and use of hydrogen more, including the purification cost can incentivise new
[61,315]. A new roadmap was developed for international and research into enhancing the endpoint application tolerance
individual countries national standardisation guidelines for hydrogen purity grade. The state-of-the-art hydrogen pu-
[13,315,321]. Therefore, a new set of norms emerged like ISO rification techniques are summarised in Table 9.
16,110 (all parts), for hydrogen generators using fuel process-
ing technologies and ISO 22,734 (all parts), for hydrogen gen-
erators using the water electrolysis process [13,315,321,322]. Innovative hydrogen cleanness index model
Hence, the choice of HPP must take into account the
hydrogen fuel purity grade required by the endpoint pathway The meaning of energy cleanness meaning in the literature is
and purification technology viability. The literature reveals an the least amount of GHG emissions associated with the LCA
enormous number of research studies on purification tech-
nologies and continues to grow [107,304,323e325]. Despite,
purification being done during the production stage or at the
Table 8 e Hydrogen grades for specific applications.
endpoint application, but the cost of purification must be
included in the HPP. This can change the cost-effectiveness of Purity (Grade) Category references
>99.9999% (>6.0) Hydrogen for Research Grade [316,317]
(R&D) Oxygen < 0.1 ppm
Water < 0.5 ppm
Table 7 e List of allowable limits for critical contaminants
Total Hydrocarbon (as
in hydrogen fuel for Fuel Cells.
CH4) < 0.5 ppm
Contaminant Allowable Limit Nitrogen < 0.5 ppm
Carbon Dioxide < 0.2 ppm
Helium (He) 300 ppm
>99.999% (>5.0) Ultra-High Purity Grade [316e320]
Nitrogen (N2) & Argon (Ar) 100 ppm
(semiconductor applications)
Water (H2O) 5 ppm
Oxygen < 2 ppm
Oxygen (O2) 5 ppm
Water < 3 ppm
Carbon Dioxide (CO2) 2 ppm
Total Hydrocarbon (as
Total Hydrocarbons 2ppm
CH4) < 0.5 ppm
Formic Acid (CH2O2) 0.2 ppm
Nitrogen < 8 ppm
Carbon Monoxide (CO) 0.2 ppm
>99.99% (>4.0) Zero Grade (Fuel Cells) [316]
Ammonia (NH3) 0.1 ppm
Total Hydrocarbon (as
Total halogenated compoundsa 0.05 ppm
CH4) < 0.5 ppm
(Halogenate ion basis)
99.99% (4.0) High Purity Grade (Fuel Cells) [319,320]
Formaldehyde (CH2O) 0.01 ppm
>99.95% (>3.5) Industrial Grade [319]
Total Sulphur (incl. H2S) 0.004 ppm
Oxygen < 10 ppm
Particles 1 mg/kg H2
Water < 34 ppm
a
Includes, for example, hydrogen bromide (HBr), hydrogen chlo- Total Hydrocarbon (as
ride (HCl), chlorine (Cl2), and organic halides (R-X). CH4) < 10 ppm
3858 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 5 ( 2 0 2 0 ) 3 8 4 7 e3 8 6 9

Table 9 e Hydrogen purification techniques.

Pathway Technology Purity (%) Recovery R&D Area Ref
Rate (%)
Membrane (Diffusion) Palladium membrane 99.99,999 99 Reduce cost [49,51,107,109,180,183,
& (Membrane Reactors) Noble metal membrane 99.8 95 Reduce working Heat 184,323,324]
Solid polymer electrolyte 92e98 >85 Purity/Recovery rate balance [108,109]
Polymer Membrane 99.5 >95 Mitigate Technical challenges [107,186]
Carbon membranes
Metaleorganic frameworks
Chemical-Catalytic Recombination/ 99.999 99 Reduce catalyst cost [326,327]
Deoxygenation Mitigate Technical challenges [109]
Noble/Non-Noble-based [323]
catalysts
Water gas shift reaction
Physical Metal hydride 99e99.99 75e95 Expensive/Simple to use [181,182]
Pressure swing adsorption 98e99.999 46e85 Enhance recovery rate [185,328e330]
Cryogenic separation 95e99.8 95 Purity/Recovery rate balance [109]
Electro-chemical Nanoporous Phosphorene NA NA Purity/Recovery rate balance [180]
membrane þ electric field [325]
ProtoniceElectronic
conducting membrane

including direct and indirect emissions of that energy (well to
end-use) [154,331,332]. Therefore, the cleanness of the HPP
determines the cleanness of energy carried (stored) in that
hydrogen [50,65,99,192,276]. Hence, the cleanness of the HPP is
determined by the life cycle cleanness of input energy, ma-
terials and equipment [17,154,252]. Thus, the hydrogen-
containing materials used to extract the hydrogen and the
catalytic energy or materials which can add GHG emissions
must be considered in any hydrogen energy cleanness
description which is called the “guarantee of origin” [331,333].
Literature reveals three colours used to distinguish be-
tween pollutant, quasi-clean and clean HPP
[48,62,78,222,235,236]. Thus, the hydrogen cleanness is
labelled by three main colours; grey, blue and green
[48,222,235,236]. The grey hydrogen is considered dirty
(polluting) even though this hydrogen produces zero-carbon-
emission at the end-use point [48,235]. Whilst, blue
hydrogen defines the CCS technology inclusive in the grey
hydrogen regardless the extraction and fugitive emission of
the fossil feedstock [48,57,222,235,237]. On the other hand,
green hydrogen refers to a renewable energy for production of
that hydrogen [48,60,235] which is then named “renewable
hydrogen” [10,11,13,15,16,35,50,60,65,77,175,176,190,
192,198,223,226,241,276,334e336]. Some other colours are
used at times in the literature like brown for brown coal
hydrogen, yellow for solar energy powered electrolysis and
purple for nuclear-powered electrolysis or thermolysis
[13,47,62,288,337].
Therefore, the current colour coding model referring to the
type of input energy of the production process rather than
how polluting or clean is that hydrogen is, fails to accurately
determine how clean is the energy stored in any produced
hydrogen [311]. Moreover, when green hydrogen is mentioned
in the literature and in public it means (renewable hydrogen)
which used zero-emissions energy [10,48,60,62,78,154]. How-
ever, the use of some RE resources like bioenergy emits GHG
such as COx, SOx and CH4 [8,252,338,339] or RE heat utilisation
which can emit N2O and NOx [88,252,340]. On the other hand,
the CCS technology can produce comparably cleaner blue
hydrogen [331,332] or can be used with some bio-renewables
to reduce GHG emissions [8,72,88]. However, the CCS energy
consumption and effectiveness in removing carbon must be
included in the total emissions.
Despite, some attempts in the literature to specify the
threshold emissions for green HPP as 4.4 kg CO2-e/kgH2
[288,331], the credit for cleaner hydrogen regardless of its
origin is not described. Furthermore, a wide range of GHG
could be emitted from the HPP but not reflected in the current
three colour coding model. Moreover, the current three colour
code does not include the depth of assessment conducted to
determine the colour coding. Hence, the authors of this paper
proposed an innovative approach using the concept of the
colour spectrum with cleanness percentage instead of a
spectral colour as illustrated in Fig. 5.
The new model has been designed to describe the per-
centage of cleanness followed by a depth level number as
shown in the right column of Fig. 5. The assessment depth
level indicates if other scopes (indirect) emission or further
depth of source and/or equipment lifecycle emission were
taken into account. Also, the contribution of production
equipment and any sub-system like purification or
compression were given an individual level in the depth of
assessment. Hence, the proposed model can determine pre-
cisely how grey is the grey hydrogen, how blue is the blue
hydrogen and how green is the green hydrogen. Authors
introduced the model as a Hydrogen Cleanness Index (HCI)
followed by the depth level number e.g. (75 Green-2)
hydrogen means that renewable energy was utilised to pro-
duce hydrogen, but it is not a zero-emission process. Instead
75% green due to some emissions associated with this pro-
cess. The number after the colour which in this example is (2)
referring to the developed model in Fig. 5, tells that indirect
GHG emission (CO2-e) associated with the production
pathway has been considered.
This innovative model needs much more work to deter-
mine the threshold levels of start and end of the spectrum for
each colour as well as the assessment depth levels and the
associated weight for each level. This will be developed,
 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 5 ( 2 0 2 0 ) 3 8 4 7 e3 8 6 9
Fig. 5 e Innovative hydrogen cleanness index (HCI), and its depth of assessment.
modelled and simulated in a separated research paper by
authors.
Discussion

Global warming is blamed on our dependence on fossil
fuels. Growing public and government awareness as well
as energy security and price stability force the shift away
from the fossil fuel economy toward a cleaner economy.

Hydrogen is an energy carrier not an energy source. The
energy used to extract hydrogen will be stored in the pro-
duced hydrogen. Hydrogen is storable, transportable and
utilisable and has gained potential as alternative energy
storage and distribution system which is known as
Hydrogen Economy.

Despite hydrogen being zero-carbon-emission energy at
the end-use point, it depends on the clean energy index
(cleanness) of the production pathway and the energy used
to produce it.

The literature reveals many reviews, case studies and
roadmaps as well as research and innovations in the R&D
field to promote the hydrogen economy and still gaining
momentum. However, the literature review shows that
most publications focused on specific parts of the
hydrogen cycle that are not interconnecting the whole
lifecycle stages.

One of the main contributions of this paper is to develop an
innovative hydrogen cycle model that has been presented
as four corners of a square-shaped integrated whole to
demonstrate the interconnection and interdependency of
these hydrogen lifecycle stages and the associated sub-
systems. Hydrogen Square (HydS) shown in Fig. 1 com-
prises four stages (square corners) which are production,
storage, safety and utilisation as well as purification and
compression as subsystems.

These subsystems can exist in one or more corners of the
HydS and must be considered as an extra cost in any
pathway selection decision.
3859

This review paper has focused on the first corner of the
HydS model in connection with the other corners and the
purification subsystem. The conclusion was that the
hydrogen production corner determines the cleanness of
any energy carried in the produced hydrogen. However, the
other HydS corners can add pollution during the round-trip
cycle of any produced hydrogen.

The literature revealed that the HPPs had been categorised
according to the process type in the mix with input energy
type and catalyst. The current categorising model did not
clearly distinguish the input energy type applied to the
different hydrogen-containing materials and type of cata-
lyst used in the process. It is a process description rather
than a pathway categorising model.

This paper proposed an innovative HPP categorising model
shown in Fig. 4, to divide the HPPs into three levels i.e.
input energy, catalyst and hydrogen-containing material.
This can describe precisely the HPP rather than the type of
process only. Table 4 has been developed to categorise the
HPPs according to the proposed model.

The hydrogen purification subsystem has been recognised
in this paper as an additive cost for any HPP selection in
connection with the other HydS corners. A list of allowable
limits for critical contaminants in hydrogen fuel for fuel
cells in Table 7 shows the necessity to consider the end-use
application in the fourth HydS corner during the techno-
economic assessment of any HPP in the first corner of the
HydS model.

The authors concluded that the cost of the hydrogen pu-
rification process must be added to the hydrogen cycle
feasibility assessment. The state-of-the-art hydrogen pu-
rification techniques were summarised in Table 9 to
highlight some promising emerging technologies which
can advantage some HPP among the classic trend of these
pathways.

The current colour coding system fails to precisely describe
the cleanness of any produced hydrogen rather than a
guarantee of origin. This raises the question of whether all
green hydrogen is cleaner than blue hydrogen? Or whether
3860 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 5 ( 2 0 2 0 ) 3 8 4 7 e3 8 6 9
using 100% renewable energy to extract hydrogen from
fossil fuel with CCS is green or blue hydrogen?

An innovative colour coding model has been proposed in
this paper to describe the percentage of cleanness of any
produced hydrogen rather than a guarantee of origin only.

The proposed Hydrogen Cleanness Index (HCI) model in
Fig. 5 has been introduced to replace the current colour
coding model to ensure the cleanness of hydrogen energy as
a percentage rather than a one colour blanket coding. Also,
this new HCI has been designed to show the deepness of the
cleanness assessment by a number to represent the level
(scope) of the assessment process. The authors of this paper
found that the new model will assure the clean energy index
(cleanness) of any imported, stored and utilised hydrogen.
Conclusion
Hydrogen is an emerging energy carrier in order to support
decarbonisation of the global energy and industrial sectors and
hence, producing hydrogen from renewable energy sources is
of prime interest today. Hydrogen production is the first corner
in the proposed HydS model which is interconnected and
interdependent on the other three corners of the HydS. The
selection of hydrogen production pathway must consider the
other main stages of the whole hydrogen energy system rep-
resented by these other three corners. Hence, hydrogen purifi-
cation must be included in the production pathway selection as
it may incur more cost and pollution depending on the other
three HydS corners to get the right trade-off with purity and
recovery inclusion. On the other hand, the cleanness of any
hydrogen is determined by the cleanness of the production
pathway even though it is zero-carbon-emission energy at the
end-use application. Therefore, guarantee of hydrogen origin
should become the most important factor in assessing any
hydrogen energy cleanness. By reviewing over 300 research
papers and industrial reports, a colour coding model was
shown to represent hydrogen origin. However, because this
failed to determine the cleanness of that hydrogen, a new
hydrogen cleanness index was presented for further investi-
gation and development. The findings of this study are ex-
pected to be used as guidelines by the governments,
policymakers, manufacturers, industrialists and utilities for
deployment of hydrogen roadmap for the future.
Acknowledgment
The authors gratefully acknowledge financial support from
Research Training Program Stipend Scholarship by Australian
Government and Murdoch University.
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